SPECIAL FEATURE: TUTORIAL Slow Heating Methods in Tandem Mass Spectrometry

McLuckey, Scott A.; Goeringer, Douglas E.

doi:10.1002/(sici)1096-9888(199705)32:5<461::aid-jms515>3.3.co;2-8

Cited by 102 publications

(153 citation statements)

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“…As CID is considered a slow heating process 26 , the reaction kinetics are such that upon dissociation, the phosphate group can actually move from its native position to another amino acid residue on the same peptide i.e., a gas-phase intramolecular transfer of phosphate 27–28 . To determine whether the observed neutral losses could actually reflect isobaric tag-enhanced scrambling of the phosphate moiety to a nearby serine or threonine, an alternative fragmentation mechanism, higher-energy collision dissociation (HCD), was examined.…”

Section: Resultsmentioning

confidence: 99%

Neutral Loss Is a Very Common Occurrence in Phosphotyrosine-Containing Peptides Labeled with Isobaric Tags

et al. 2016

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While developing a multiplexed phosphotyrosine peptide quantification assay, an unexpected observation was made – significant neutral loss from phosphotyrosine (pY) containing peptides. Using a 2000-member peptide library, we sought to systematically investigate this observation by comparing unlabeled peptides with the two highest-plex isobaric tags (iTRAQ8 and TMT10) across CID, HCD and ETD fragmentation using high resolution high mass accuracy Orbitrap instrumentation. We found pY peptide neutral loss behavior was consistent with reduced proton mobility, and does not occur during ETD. The site of protonation at the peptide N-terminus changes from a primary to a tertiary amine as a result of TMT labeling which would increase the gas phase basicity and reduce proton mobility at this site. This change in fragmentation behavior has implications during instrument method development and interpretation of MS/MS spectra, and therefore ensuing follow-up studies. We show how sites not localized to tyrosine by search and site localization algorithms can be confidently re-assigned to tyrosine using neutral loss and phosphotyrosine immonium ions. We believe these findings will be of general interest to those studying pY signal transduction using isobaric tags.

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Section: Resultsmentioning

confidence: 99%

Neutral Loss Is a Very Common Occurrence in Phosphotyrosine-Containing Peptides Labeled with Isobaric Tags

et al. 2016

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“…This is very similar to the energy transfer process in CID. 84,85 However, in contrast to CID, collisional activation under the QE condition does not result in significant ion fragmentation. From the underlying QE distribution, the relative fragment ion intensities can be predicted.…”

Section: Resultsmentioning

confidence: 99%

Populations of Metal-Glycan Structures Influence MS Fragmentation Patterns

Zhu

Glover

Shi

et al. 2014

J. Am. Soc. Mass Spectrom.

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The structures and collision-induced dissociation (CID) fragmentation patterns of the permethylated glycan Man5GlcNAc2 are investigated by a combination of hybrid ion mobility spectrometry (IMS), mass spectrometry (MS), and MS/MS techniques. IMS analysis of eight metal-adducted glycans ([Man5GlcNAc2+M]2+, where M = Mn, Fe, Co, Ni, Cu, Mg, Ca, and Ba) shows distinct conformer patterns. These conformers appear to arise from individual metals binding at different sites on the glycan. Fragmentation studies suggest that these different binding sites influence the CID fragmentation patterns. This paper describes a series of separation, activation, and fragmentation studies that assess which fragments arise from each of the different gas-phase conformer states. Comparison of the glycan distributions formed under gentle ionization conditions with those obtained after activation of the gas-phase ions suggests that these conformer binding states also appear to exist in solution.

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“…Mass spectrometric characterization of lipids began with electron ionization (EI) [7–9] via GC-interfaces, but most current research now relies on low-energy collisional induced dissociation (CID) [10–13] using matrix-assisted laser desorption ionization (MALDI) or atmospheric ion sources like electrospray ionization (ESI), APCI and atmospheric pressure (AP)-MALDI. The fragmentation products of glycerolipids are normally restricted to [M+Y-R x-1 CO 2 H] + , [M+Y-R x-1 CHC=O] + , where R corresponds to the sn-1 or sn-2 fatty acid chain from which the fragment originated, and Y is the charging adduct, such as Na + or H + .…”

Section: Introductionmentioning

confidence: 99%

Radical-induced fragmentation of phospholipid cations using metastable atom-activated dissociation mass spectrometry (MAD-MS)

Deimler

Sander²,

Jackson

2015

International Journal of Mass Spectrometry

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The fragmentation pattern of several protonated 1+ phosphatidylcholines (PCs) were studied using low energy collision induced dissociation (CID) and helium metastable atom-activated dissociation (He-MAD). He-MAD of the protonated compounds produced a dominant phosphocholine head group at m/z 184 as well as typical sn-1 and sn-2 glycerol fragments such as [M+H–Rx-1CHC=O]+ and [M+H-Rx-1CO2H]+. Within the aliphatic chain, He-MAD showed fragments consistent with high-energy collision induced dissociation (HE-CID) and products/pathways consistent with Penning ionization of the 1+ precursor ions to their respective radical dications. These Penning ionization products included both singly and doubly charged radical fragments, and the fragment ions are related to the number and position of double bonds in the acyl chains. Fragments created through HE-CID-like fragmentation followed classic charge remote fragmentation pathways including ladder-like fragmentation along the acyl chain, except for additional or missing peaks due to predictable rearrangement reactions. He-MAD therefore shows utility in being able to effectively fragment singly charged lipids into a variety of useful product ions using both radical and high-energy processes in the confines of a 3D ion trap.

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SPECIAL FEATURE: TUTORIAL Slow Heating Methods in Tandem Mass Spectrometry

Cited by 102 publications

References 0 publications

Neutral Loss Is a Very Common Occurrence in Phosphotyrosine-Containing Peptides Labeled with Isobaric Tags

Neutral Loss Is a Very Common Occurrence in Phosphotyrosine-Containing Peptides Labeled with Isobaric Tags

Populations of Metal-Glycan Structures Influence MS Fragmentation Patterns

Radical-induced fragmentation of phospholipid cations using metastable atom-activated dissociation mass spectrometry (MAD-MS)

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